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<p>Biological pretreatment can significantly alter biomass structure and thereby influence its thermochemical conversion. However, the structural evolution of biomass during long-term pretreatment and its impact on pyrolysis behavior remain poorly understood. Here, paulownia wood was pretreated with <i>Phanerochaete chrysosporium</i> for 90&#xa0;days, revealing for the first time a three-stage structural evolution during pretreatment—degradation, reorganization, and stabilization. Stage I (0–30&#xa0;days): Hemicellulose degradation predominated, accompanied by oxidative modification of lignin side chains and cleavage of lignin–carbohydrate complex (LCC) linkages, exposing amorphous cellulose, leading to an increased crystallinity index (CrI). Correspondingly, pyrolysis products showed significant increases in aldehydes (13.76–22.41%), together with increased phenolic yield and a 32.84% increase in the guaiacyl-to-syringyl (G/S) ratio. Stage II (30–60&#xa0;days): Lignin structural reorganization became dominant through phenoxy radical coupling, promoting lignin crosslinking and enrichment, while continued degradation further eroded amorphous cellulose, resulting in a peak CrI (11.19%) and increased char yield (4.70%). Stage III (60–90&#xa0;days): Structural evolution was governed by lignin reconstruction and cellulose degradation. Further lignin condensation produced crosslinked aromatic structures, leading to a decreased CrI and stabilized pyrolysis behavior. Overall, biological pretreatment progressively promoted deoxygenation and aromatic enrichment of the biomass structure, resulting in a shift in pyrolysis products from oxygenated compounds toward aromatic-rich species with enhanced char formation. These findings demonstrate that structural evolution during long-term biological pretreatment determines the pyrolysis behavior and pathways of biomass.</p>

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Selective degradation-induced structural evolution and pyrolysis behavior of biomass during long-term biological pretreatment

  • 期刊论文

  • 发表日期：

    2026年7月7日

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  • Fengqi Cai,
  • Linlin Yi,
  • Kaiyuan Li,
  • Shaohua Hu,
  • Wenhao Kong,
  • Yuxuan Xiao,
  • Zhuoma Zhang,
  • Xujuan Wu,
  • Zhanwen Chen,
  • Cheng Zhang,
  • Xian Li,
  • Xianzhe Liu

摘要

Biological pretreatment can significantly alter biomass structure and thereby influence its thermochemical conversion. However, the structural evolution of biomass during long-term pretreatment and its impact on pyrolysis behavior remain poorly understood. Here, paulownia wood was pretreated with Phanerochaete chrysosporium for 90 days, revealing for the first time a three-stage structural evolution during pretreatment—degradation, reorganization, and stabilization. Stage I (0–30 days): Hemicellulose degradation predominated, accompanied by oxidative modification of lignin side chains and cleavage of lignin–carbohydrate complex (LCC) linkages, exposing amorphous cellulose, leading to an increased crystallinity index (CrI). Correspondingly, pyrolysis products showed significant increases in aldehydes (13.76–22.41%), together with increased phenolic yield and a 32.84% increase in the guaiacyl-to-syringyl (G/S) ratio. Stage II (30–60 days): Lignin structural reorganization became dominant through phenoxy radical coupling, promoting lignin crosslinking and enrichment, while continued degradation further eroded amorphous cellulose, resulting in a peak CrI (11.19%) and increased char yield (4.70%). Stage III (60–90 days): Structural evolution was governed by lignin reconstruction and cellulose degradation. Further lignin condensation produced crosslinked aromatic structures, leading to a decreased CrI and stabilized pyrolysis behavior. Overall, biological pretreatment progressively promoted deoxygenation and aromatic enrichment of the biomass structure, resulting in a shift in pyrolysis products from oxygenated compounds toward aromatic-rich species with enhanced char formation. These findings demonstrate that structural evolution during long-term biological pretreatment determines the pyrolysis behavior and pathways of biomass.